A quantum dynamics method for excited electrons in molecular aggregate system using a group diabatic Fock matrix

TL;DR

This paper presents a new quantum dynamics method using a group diabatic Fock matrix to analyze excited electron behavior in molecular aggregates, considering light-electron interactions for energy conversion applications.

Contribution

The paper introduces a practical scheme for excited electron dynamics in molecular systems using a local group diabatic Fock representation, enabling detailed analysis of local excitations and electron transfer processes.

Findings

Applied to a naphthalene-TCNE dimer and a 20-mer ethylene circle.

Enabled intuitive understanding of electron transfer mechanisms.

Incorporated light-electron coupling into the dynamics analysis.

Abstract

We introduce a practical calculation scheme for the description of excited electron dynamics in molecular aggregated systems within a locally group diabatic Fock representation. This scheme makes it easy to analyze the interacting time-dependent excitations of local sites in complex systems. In addition, light-electron couplings are considered. The present scheme is intended for investigations on the migration dynamics of excited electrons in light-energy conversion systems. The scheme was applied to two systems: a naphthalene(NPTL)-tetracyanoethylene(TCNE) dimer and a 20-mer circle of ethylene molecules. Through local group analyses of the dynamical electrons, we obtained an intuitive understanding of the electron transfers between the monomers.